Award Abstract # 1553987
CAREER: Understanding the Roles of Strain and Mass Disorder on Fundamental Thermal Transport Processes in Two-Dimensional Materials
| NSF Org: | CBET |
| Recipient: | |
| Initial Amendment Date: | February 29, 2016 |
| Latest Amendment Date: | March 16, 2020 |
| Award Number: | 1553987 |
| Award Instrument: | Standard Grant |
| Program Manager: | Sumanta Acharya sacharya@nsf.gov (703)292-4509 CBET Div Of Chem, Bioeng, Env, & Transp Sys ENG Directorate For Engineering |
| Start Date: | March 1, 2016 |
| End Date: | February 28, 2019(Estimated) |
| Total Intended Award Amount: | $500,000.00 |
| Total Awarded Amount to Date: | $550,000.00 |
| Funds Obligated to Date: | FY 2017 = $50,000.00 |
| History of Investigator: |
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| Recipient Sponsored Research Office: | 438 WHITNEY RD EXTENSION UNIT 11 STORRS CT US 06269-9018 (860)486-3622 |
| Sponsor Congressional District: | |
| Primary Place of Performance: | 191 Auditorium Road, Unit 3139 Storrs CT US 06269-3139 |
| Primary Place of Performance Congressional District: | |
| Unique Entity Identifier (UEI): | |
| Parent UEI: | |
| NSF Program(s): | TTP-Thermal Transport Process, IUCRC-Indust-Univ Coop Res Ctr |
| Primary Program Source: | 01001718DBNSF RESEARCH & RELATED ACTIVIT |
| Program Reference Code(s): | |
| Program Element Code(s): | |
| Award Agency Code: | 4900 |
| Fund Agency Code: | 4900 |
| Assistance Listing Number(s): | 47.041 |
ABSTRACT The research objective of this proposal is to determine the fundamental nature of elastic strain and mass disorder on thermal transport in low-dimensional materials using technologically-critical 2D materials in order to enable their widespread adoption in flexible electronic technologies. Investigating the nature of elastic strain and mass disorder on thermal transport in low-dimensional materials using technologically-critical 2D materials in heavy, semiconducting quasi-2D layered transition metal dichalcogenides (LTMDs) MoS2 and WS2, as well as in light, metallic truly-2D graphene, will yield insight into controversial phenomena such as divergently increasing thermal conductivity and coherent phonon transport. An innovative approach here is to develop a metrology technique using a micro-thermometry device and in situ transmission electron microscopy (TEM) to probe heat dissipation mechanisms in the presence of mechanical stimulus. This work will provide a conceptual advance in knowledge concerning the effect of mechanical stimulus and isotopic disorder on heat transfer in technologically-critical 2D materials. The outcome of this work will enable the development of new and widely applicable strain and isotopic engineering strategies to alter thermal transport processes in low-dimensional systems, in addition to solving critical questions needed for the design of flexible electronic technologies. Through this project, a new TEM-based metrology tool to quantify the elastic strain effect on the thermal conductivity of low-dimensional materials will be developed, and a Raman spectroscopic technique to probe both long-wavelength and dispersive phonons will be further developed. These new techniques will allow the effects of strain and isotopic disorder on thermal transport and phonon dispersions in 2D systems with different structural characteristics to be identified. Especially promising, the methods and outcome of this study will be generally applicable to a wide class of low-dimensional materials. Furthermore, through the development of a mentor/teacher/student nucleus in nanoscale thermal transport, state-of-the-art active experimental research and educational experiences for a unique group of student researchers and pre-college educators will be implemented and evaluated. Several Ph.D. students and numerous undergraduate and pre-college students will be mentored through this project. Hands-on educational modules created through integration of this project with the NSF RET program will extend its impact into K-12 science curriculum. The proposed activities will broaden opportunities and increase accessibility of experimental nanotechnology research to underrepresented populations and the disabled in Connecticut.
Technologies based on two-dimensional (2D) materials offer size, weight, power, and cost advantages not currently achievable using traditional materials. These attributes combined with the ability to tune the properties of these materials at the atomic scale makes them ideal for envisioned flexible nanoelectronic and ultra-high frequency applications. This project will generate fundamental knowledge of energy transport in 2D materials critical for advanced nanoelectronic device technologies. These beyond next-generation technologies have the potential to foster a revolution in computing comparable to the transition from the vacuum tube to the transistor. The outcomes of this project are likely to have a catalytic effect on the thermal engineering community as very little is known regarding the fundamental nature of a material's thermal response to elastic stimulus and mass disorder, effects which have been predicted to offer unprecedented control over intrinsic physico-chemical properties. Large changes have been predicted for thermal transport in the presence of elastic strain, and whether this should be exploited (strain enhanced devices) or prevented (strain robust devices) is a key remaining scientific question. Since no accepted technique exists in which to probe strain-effects on heat transfer mechanisms in nanomaterials, resolving this issue is a limiting challenge for the progress of nanoelectronic technologies. Furthermore, isotopic mass disorder is beginning to be understood as a tool that can be used to beneficially alter thermal transport mechanisms, thereby enabling higher power output in nanoelectronic devices. Yet understanding of the effect in low-dimensional materials is controversial, especially in light of recent phonon transport models invoking coherency effects.
PUBLICATIONS PRODUCED AS A RESULT OF THIS RESEARCH
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Wu, Wei and Wang, Jin and Ercius, Peter and Wright, Nicomario Courtney and Leppert-Simenauer, Danielle Marie and Burke, Robert A. and Dubey, Madan and Dongare, Avinash M. and Pettes, Michael Thompson "Giant Mechano-Optoelectronic Effect in an Atomically Thin Semiconductor" Nano Letters , 2018 10.1021/acs.nanolett.7b05229 Citation Details
Palmieri, Alessandro and Yazdani, Sajad and Kashfi-Sadabad, Raana and Karakalos, Stavros G. and Pettes, Michael Thompson and Mustain, William Earl "Cobalt Doping as a Pathway to Stabilize the Solid-State Conversion Chemistry of Manganese Oxide Anodes in Li-Ion Batteries" The Journal of Physical Chemistry C , 2018 10.1021/acs.jpcc.8b00403 Citation Details
Yazdani, Sajad and Kim, Hyun-Young and Pettes, Michael T "A high temperature instrument for consecutive measurements of thermal conductivity, electrical conductivity, and Seebeck coefficient" Journal of Heat Transfer , 2019 10.1115/1.4043572 Citation Details
Yazdani, Sajad and Kashfi-Sadabad, Raana and Palmieri, Alessandro and Mustain, William E and Thompson Pettes, Michael "Effect of cobalt alloying on the electrochemical performance of manganese oxide nanoparticles nucleated on multiwalled carbon nanotubes" Nanotechnology , v.28 , 2017 10.1088/1361-6528/aa6329 Citation Details
Yazdani, Sajad and Kashfi-Sadabad, Raana and Morales-Acosta, Mayra Daniela and Montaño, Raul David and Vu, Tuoc Ngoc and Tran, Huan Doan and Zhou, Menghan and Liu, Yufei and He, Jian and Thompson Pettes, Michael "Thermal transport in phase-stabilized lithium zirconate phosphates" Applied Physics Letters , v.117 , 2020 10.1063/5.0013716 Citation Details
Pettes, Michael Thompson and Kim, Jaehyun and Wu, Wei and Bustillo, Karen C. and Shi, Li "Thermoelectric transport in surface- and antimony-doped bismuth telluride nanoplates" APL Materials , v.4 , 2016 10.1063/1.4955400 Citation Details
Yazdani, Sajad and Kim, Hyun-Young and Pettes, Michael Thompson "Uncertainty analysis of axial temperature and Seebeck coefficient measurements" Review of Scientific Instruments , v.89 , 2018 10.1063/1.5023909 Citation Details
Wu, Jason Yingzhi and Wu, Wei and Pettes, Michael Thompson "Ultra-high resolution steady-state micro-thermometry using a bipolar direct current reversal technique" Review of Scientific Instruments , v.87 , 2016 10.1063/1.4962714 Citation Details
Hernandez, Jose A. and Ruiz, Angel and Fonseca, Luis F. and Pettes, Michael T. and Jose-Yacaman, Miguel and Benitez, Alfredo "Thermoelectric properties of SnSe nanowires with different diameters" Scientific Reports , v.8 , 2018 10.1038/s41598-018-30450-5 Citation Details
Yazdani, Sajad and Pettes, Michael Thompson "Nanoscale self-assembly of thermoelectric materials: A review of chemistry-based approaches" Nanotechnology , 2018 10.1088/1361-6528/aad673 Citation Details
Wu, Wei and Morales-Acosta, Mayra Daniela and Wang, Yongqiang and Pettes, Michael Thompson "Isotope Effect in Bilayer WSe 2" Nano Letters , 2019 10.1021/acs.nanolett.8b04269 Citation Details
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PROJECT OUTCOMES REPORT
Disclaimer
This Project Outcomes Report for the General Public is displayed verbatim as submitted by the Principal Investigator (PI) for this award. Any opinions, findings, and conclusions or recommendations expressed in this Report are those of the PI and do not necessarily reflect the views of the National Science Foundation; NSF has not approved or endorsed its content.
This highly successful project produced 18 peer reviewed publications (many with undergraduate co-authors), 2 doctoral theses, 2 patent applications by the principal investigator, and exposed a multitude of undergraduate students to cutting-edge scientific research in the classroom and the laboratory. Project objectives were completed in only 36 months and were well under budget. The main findings of the study were related to strain and isotopic control over transport properties in two dimensional semiconductors.
The team made the world's first demonstration of isotopic purification in a 2D transition metal dichalcogenide and its induced changes in the electronic band structure and phonon spectra, including an unexpected change in the light emission spectra. The ability to tune electron and phonon energies intrinsically through isotope engineering opens the door to new developments in microelectronics as well as quantum photon sources based on 2D materials. The proposed mechanism is the effect of isotopic purification on atomic mass, which leads to a decrease in phonon energies and ultimately a difference in electronic band gap renormalization energy.
In search of the effect of strain on emergent phonon and other properties in these materials, the team also discovered a method to create spatially localized quantum emission sites in a wafer-scale transition metal dichalcogenide film. A new route to engineer spatially localized quantum emission in the 750-800 nm regime using wafer-scale few-layer WSe2 and ultra-sharp SiO2 tips was reported, which brings advantages in spectral stability and offers an order of magnitude increase in lifetime compared with free and point defect exciton recombination rates. This discovery contributes to the push for beyond lab-scale quantum materials needed for all-optical quantum information science.
The project also included a supplementary award to stimulate graduate student research at a U.S. Department of Energy national laboratory (Lawrence Berkeley National Laboratory) which resulted in the first discovery of a giant-strain response in a 2D material. The team reported that a six-atom thick bilayer of tungsten diselenide exhibited a 100-fold increase in photoluminescence when it was subjected to strain. The material had never exhibited such photoluminescence before. The findings are important in that they mark the first time scientists have been able to conclusively show that atomically thin materials can be mechanically manipulated to enhance their performance. The process the team used to achieve the outcome is also significant in that it offers a reliable new methodology for measuring the impact of strain on ultrathin materials, something that has been difficult to do and a hindrance to innovation.
Last Modified: 07/07/2020
Modified by: MichaelTPettes
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This is the first demonstration of isotopic purification in a 2D transition metal dichalcogenide. Upper left graphic is the naturally abundant WSe2. Lower right graphic is the isotopically pure WSe2. A blue-shift of light emission occurs in the isotopically pure sample.
Daniel Edward Judge Jr. (Los Alamos National Laboratory)
Copyrighted
MichaelTPettes
Isotopically pure thin-film exhibits unexpected blue-shift
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Scanning electron micrograph of the array used to create deterministic single photon sources in epitaxial tungsten diselenide. Inset shows the Hanbury-Brown Twiss interferometry measurement proving quantum emission.
Michael Pettes
Copyrighted
MichaelTPettes
Strain Control of Deterministic Quantum Emission in an Epitaxial 2D Host
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Nicomario Wright and Danielle Leppert-Simenauer work on precursor prep (left) and 2D materials growth using a tube furnace in the Pettes Lab. Nico came to the project through the Ronald E. McNair program and Danielle came through the NSF REU program, both are co-authors in peer-reviewed publications
University of Connecticut Ronald E. McNair Program
Copyrighted
MichaelTPettes
2D Materials Research Brings Undergrads Together in Science
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